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Explaining global surface aerosol number concentrations in terms of primary emissions and particle formation

Spracklen, D. V. and Carslaw, K. S. and Merikanto, J. and Mann, G. W. and Reddington, C. L. and Pickering, S. and Ogren, J. A. and Andrews, E. and Baltensperger, U. and Weingartner, E. and Boy, M. and Kulmala, M. and Laakso, L. and Lihavainen, H.Finnish Meteorol. Inst., and Kivekäs, N. and Komppula, M. and Mihalopoulos, N. and Kouvarakis, G. and Jennings, S. G. and O'Dowd, C. and Birmili, W. and Wiedensohler, A. and Weller, R. and Gras, J. and Laj, P. and Sellegri, K. and Bonn, B. and Krejci, R. and Laaksonen, A. and Hamed, A. and Minikin, A. and Harrison, R. M. and Talbot, R. and Sun, J. (2010) Explaining global surface aerosol number concentrations in terms of primary emissions and particle formation. Atmospheric Chemistry and Physics, 10, pp. 4775-4793. Copernicus Publications. doi: 10.5194/acp-10-4775-2010.

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Official URL: http://www.atmos-chem-phys.net/10/4775/2010/acp-10-4775-2010.html

Abstract

We synthesised observations of total particle number (CN) concentration from 36 sites around the world. We found that annual mean CN concentrations are typically 300� 2000 cm�3 in the marine boundary layer and free troposphere (FT) and 1000�10 000 cm�3 in the continental boundary layer (BL). Many sites exhibit pronounced seasonality with summer time concentrations a factor of 2�10 greater than wintertime concentrations. We used these CN observations to evaluate primary and secondary sources of particle number in a global aerosol microphysics model. We found that emissions of primary particles can reasonably reproduce the spatial pattern of observed CN concentration (R2=0.46) but fail to explain the observed seasonal cycle (R2=0.1). The modeled CN concentration in the FT was biased low (normalised mean bias, NMB=�88%) unless a secondary source of particles was included, for example from binary homogeneous nucleation of sulfuric acid and water (NMB=�25%). Simulated CN concentrations in the continental BL were also biased low (NMB=�74%) unless the number emission of anthropogenic primary particles was increased or a mechanism that results in particle formation in the BL was included. We ran a number of simulations where we included an empirical BL nucleation mechanism either using the activation-type mechanism (nucleation rate, J , proportional to gas-phase sulfuric acid concentration to the power one) or kinetic-type mechanism (J proportional to sulfuric acid to the power two) with a range of nucleation coefficients. We found that the seasonal CN cycle observed at continental BL sites was better simulated by BL particle formation (R2=0.3) than by increasing the number emission from primary anthropogenic sources (R2=0.18). The nucleation constants that resulted in best overall match between model and observed CN concentrations were consistent with values derived in previous studies from detailed case studies at individual sites. In our model, kinetic and activation-type nucleation parameterizations gave similar agreement with observed monthly mean CN concentrations.

Item URL in elib:https://elib.dlr.de/64198/
Document Type:Article
Title:Explaining global surface aerosol number concentrations in terms of primary emissions and particle formation
Authors:
AuthorsInstitution or Email of AuthorsAuthor's ORCID iDORCID Put Code
Spracklen, D. V.Univ. of Leeds, UKUNSPECIFIEDUNSPECIFIED
Carslaw, K. S.Univ. of Leeds, UKUNSPECIFIEDUNSPECIFIED
Merikanto, J.Univ. of Leeds, UKUNSPECIFIEDUNSPECIFIED
Mann, G. W.Univ. of Leeds, UKUNSPECIFIEDUNSPECIFIED
Reddington, C. L.Univ. of Leeds, UKUNSPECIFIEDUNSPECIFIED
Pickering, S.Univ. of Leeds, UKUNSPECIFIEDUNSPECIFIED
Ogren, J. A.NOAA/ESRL Global Monitoring Division, Boulder, CO, USAUNSPECIFIEDUNSPECIFIED
Andrews, E.NOAA/ESRL Global Monitoring Division, Boulder, CO, USAUNSPECIFIEDUNSPECIFIED
Baltensperger, U.Lab. of Atmospheric Chemistry, Villigen, CHUNSPECIFIEDUNSPECIFIED
Weingartner, E.Lab. of Atmospheric Chemistry, Villigen, CHUNSPECIFIEDUNSPECIFIED
Boy, M.Univ. of Helsinki, FINUNSPECIFIEDUNSPECIFIED
Kulmala, M.Univ. of Helsinki, FINUNSPECIFIEDUNSPECIFIED
Laakso, L.Univ. of Helsinki, FINUNSPECIFIEDUNSPECIFIED
Lihavainen, H.Finnish Meteorol. Inst.,Finnish Meteorol. Inst., Helsinki, FINUNSPECIFIEDUNSPECIFIED
Kivekäs, N.Finnish Meteorol. Inst., Helsinki, FINUNSPECIFIEDUNSPECIFIED
Komppula, M.Finnish Meteorol. Inst., Helsinki, FINUNSPECIFIEDUNSPECIFIED
Mihalopoulos, N.Univ. of Crete, Heraklion, GRUNSPECIFIEDUNSPECIFIED
Kouvarakis, G.Univ. of Crete, Heraklion, GRUNSPECIFIEDUNSPECIFIED
Jennings, S. G.National Univ. of Ireland, Galway, IRUNSPECIFIEDUNSPECIFIED
O'Dowd, C.National Univ. of Ireland, Galway, IRUNSPECIFIEDUNSPECIFIED
Birmili, W.Leibniz Institute for Tropospheric Research, LeipzigUNSPECIFIEDUNSPECIFIED
Wiedensohler, A.Leibniz Institute for Tropospheric Research, LeipzigUNSPECIFIEDUNSPECIFIED
Weller, R.Alfred Wegener Institute, BremerhavenUNSPECIFIEDUNSPECIFIED
Gras, J.CSIRO Marine and Atmospheric Research, Aspendale, Victoria, AUUNSPECIFIEDUNSPECIFIED
Laj, P.Univ. Grenoble, FUNSPECIFIEDUNSPECIFIED
Sellegri, K.Univ. Clermont-Ferrand/CNRS, Clermont-Ferrand, FUNSPECIFIEDUNSPECIFIED
Bonn, B.J. W. Goethe Univ., Frankfurt/MainUNSPECIFIEDUNSPECIFIED
Krejci, R.Stockholm Univ., SUNSPECIFIEDUNSPECIFIED
Laaksonen, A.Finnish Meteorol. Inst., Helsinki, FINUNSPECIFIEDUNSPECIFIED
Hamed, A.Univ. of Eastern Finland, Kuopio, FINUNSPECIFIEDUNSPECIFIED
Minikin, A.UNSPECIFIEDUNSPECIFIEDUNSPECIFIED
Harrison, R. M.Univ. of Birmingham, UKUNSPECIFIEDUNSPECIFIED
Talbot, R.Univ. of New Hampshire, Durham, NH, USAUNSPECIFIEDUNSPECIFIED
Sun, J.Chinese Academy of Meteoroi. Sciences, Beijing, CHNUNSPECIFIEDUNSPECIFIED
Date:26 May 2010
Journal or Publication Title:Atmospheric Chemistry and Physics
Refereed publication:Yes
Open Access:Yes
Gold Open Access:Yes
In SCOPUS:Yes
In ISI Web of Science:Yes
Volume:10
DOI:10.5194/acp-10-4775-2010
Page Range:pp. 4775-4793
Publisher:Copernicus Publications
Status:Published
Keywords:aerosol, troposphere, CN, particle formation
HGF - Research field:Aeronautics, Space and Transport (old)
HGF - Program:Space (old)
HGF - Program Themes:W EO - Erdbeobachtung
DLR - Research area:Space
DLR - Program:W EO - Erdbeobachtung
DLR - Research theme (Project):W - Vorhaben Atmosphären- und Klimaforschung (old)
Location: Oberpfaffenhofen
Institutes and Institutions:Institute of Atmospheric Physics > Atmospheric Trace Species
Deposited By: Minikin, Dr.rer.nat. Andreas
Deposited On:01 Jun 2010 13:45
Last Modified:02 May 2019 14:03

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